By addressing fundamental issues related to soft, LC-based materials on multiple length scales via the integration of complementary experimental and theoretical tools, IRG 3 provides a foundation of knowledge with broad potential for impact on the design of hierarchical and active soft materials. Key fundamental issues IRG 3 investigates include the equilibrium and the non-equilibrium, dynamic behaviors of molecules at interfaces of anisotropic soft materials, interfacial ionic phenomena in LC systems, dynamic mechanical and transport properties of several classes of LC gels, including concepts of molecular frustration and surface-driven ordering transitions, and the structure and energetics of the cores of LC defects, including cores that host adsorbates. The challenge of designing these complex LC material systems is addressed by IRG 3 through the development of new experimental techniques, multi-scale theory and simulation, and new methods of synthesis and processing.